Performance of ZrO2-supported Nb- and W-oxide in the gas-phase dehydration of glycerol to acrolein

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Performance of ZrO2-supported Nb- and W-oxide in the gas-phase dehydration of glycerol to acrolein. / Massa, Mariano; Andersson, Arne; Finocchio, Elisabetta; Busca, Guido; Lenrick, Filip; Wallenberg, Reine.

In: Journal of Catalysis, Vol. 297, 2013, p. 93-109.

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Massa, Mariano ; Andersson, Arne ; Finocchio, Elisabetta ; Busca, Guido ; Lenrick, Filip ; Wallenberg, Reine. / Performance of ZrO2-supported Nb- and W-oxide in the gas-phase dehydration of glycerol to acrolein. In: Journal of Catalysis. 2013 ; Vol. 297. pp. 93-109.

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TY - JOUR

T1 - Performance of ZrO2-supported Nb- and W-oxide in the gas-phase dehydration of glycerol to acrolein

AU - Massa, Mariano

AU - Andersson, Arne

AU - Finocchio, Elisabetta

AU - Busca, Guido

AU - Lenrick, Filip

AU - Wallenberg, Reine

PY - 2013

Y1 - 2013

N2 - Gas-phase dehydration of glycerol to acrolein is studied over tungsten and niobium oxide supported on monoclinic zirconia. Supported tungsten oxide is slightly better than supported niobia with initial yields to acrolein around 78% and 75%, respectively, at complete conversion of glycerol. No synergy is observed using mixed structures with W and Nb. The addition of oxygen to the feed has almost no effect on the yield to acrolein but reduces the deactivation rate. XPS and HRTEM imaging reveals that deactivation is due to formation of an amorphous layer on the surface, consisting of adsorbed high-boiling compounds and coke. Regeneration experiments show that the catalysts are effectively regenerated in flowing air. Characterization of the catalysts with Raman, FTIR, and pyridine adsorption reveals that the active surface structure is polymeric oxide exposing W=O and/or Nb=O species and Bronsted acidic W OH and/or Nb OH groups. The results show that Bronsted acidic sites are required for the catalyst to be active and selective to acrolein. (c) 2012 Elsevier Inc. All rights reserved.

AB - Gas-phase dehydration of glycerol to acrolein is studied over tungsten and niobium oxide supported on monoclinic zirconia. Supported tungsten oxide is slightly better than supported niobia with initial yields to acrolein around 78% and 75%, respectively, at complete conversion of glycerol. No synergy is observed using mixed structures with W and Nb. The addition of oxygen to the feed has almost no effect on the yield to acrolein but reduces the deactivation rate. XPS and HRTEM imaging reveals that deactivation is due to formation of an amorphous layer on the surface, consisting of adsorbed high-boiling compounds and coke. Regeneration experiments show that the catalysts are effectively regenerated in flowing air. Characterization of the catalysts with Raman, FTIR, and pyridine adsorption reveals that the active surface structure is polymeric oxide exposing W=O and/or Nb=O species and Bronsted acidic W OH and/or Nb OH groups. The results show that Bronsted acidic sites are required for the catalyst to be active and selective to acrolein. (c) 2012 Elsevier Inc. All rights reserved.

KW - Glycerol

KW - Dehydration

KW - Oxidative dehydration

KW - Acrolein

KW - Acrylic acid

KW - WO3/ZrO2

KW - Nb2O5/ZrO2

KW - Nb-W-O/ZrO2

KW - Deactivation

KW - Regeneration

U2 - 10.1016/j.jcat.2012.09.021

DO - 10.1016/j.jcat.2012.09.021

M3 - Article

VL - 297

SP - 93

EP - 109

JO - Journal of Catalysis

T2 - Journal of Catalysis

JF - Journal of Catalysis

SN - 1090-2694

ER -